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Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
Published on: April 10, 2018
Auene-Supported Transition-Metal Single-Atom Catalysts for Promising Electrocatalytic Nitrogen Reduction
Luxuan Huang1, Jingyao Liu2, Zhong-Min Su1,2
1School of Chemistry and Environmental Engineering, Changchun University of Science and Technology, Changchun, China.
None:
The electrochemical nitrogen reduction reaction (NRR) provides a sustainable route to ammonia synthesis, but its efficiency is hindered by the inert N≡N bond and competing hydrogen evolution reaction (HER). Herein, we systematically screened 25 transition-metal (TM) single-atom catalysts (SACs) supported on goldene, denoted as TM@Auene, using density functional theory (DFT). Sixteen TM@Auene systems capable of end-on N2 adsorption were evaluated across distal, alternating, and mixed NRR pathways. Mo@Auene and Re@Auene exhibited high NRR catalytic activity with low limiting potentials of -0.04 and -0.10 V, respectively, associated with effective N2 activation through synergistic σ-donation and π*-back-donation. A volcano-type relationship was established between NRR activity and occupied d-electron number, positioning Mo and Re near the optimum. HER competition was assessed, with Nb@Auene, Mo@Auene, W@Auene, Re@Auene, and Os@Auene showing favorable NRR selectivity. For Mo@Auene and Re@Auene, Pourbaix diagram analysis and ab initio molecular dynamics (AIMD) simulations provide preliminary support for electrochemical stability and short-timescale structural integrity under NRR-relevant conditions. These results identify Mo@Auene as a promising NRR candidate and highlight Auene-supported SACs as a descriptor-guided platform for catalyst design.
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